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University of Southampton Research Repository University of Southampton Research Repository Copyright © and Moral Rights for this thesis and, where applicable, any accompanying data are retained by the author and/or other copyright owners. A copy can be downloaded for personal non-commercial research or study, without prior permission or charge. This thesis and the accompanying data cannot be reproduced or quoted extensively from without first obtaining permission in writing from the copyright holder/s. The content of the thesis and accompanying research data (where applicable) must not be changed in any way or sold commercially in any format or medium without the formal permission of the copyright holder/s. When referring to this thesis and any accompanying data, full bibliographic details must be given, e.g. Thesis: Elizabeth Sarah Marsden (2019) "The Role and Implications of Mineral Associations in Organic Carbon Preservation", University of Southampton, Faculty of Environmental and Life Sciences, School of Ocean and Earth Science PhD Thesis, pagination. University of Southampton Faculty of Environmental and Life Sciences Ocean and Earth Science The Role and Implications of Mineral Associations in Organic Carbon Preservation DOI by Elizabeth Sarah Marsden ORCID ID 0000-0002-4150-6636 Thesis for the degree of Doctor of Philosophy December 2019 University of Southampton Abstract Faculty of Environmental and Life Sciences Ocean and Earth Science Thesis for the degree of Doctor of Philosophy The Role and Implications of Mineral Associations in Organic Carbon Preservation by Elizabeth Sarah Marsden Organic matter-mineral interactions are a key part of the global carbon cycle, facilitating the preservation of organic matter that helps remove CO2 from the atmosphere and allow for the build-up of oxygen in the ocean-atmosphere system. In this project, chemical standards were added to clay and iron minerals (kaolinite, bentonite and goethite), to investigate the effect of organic matter and mineral type on sorption, as well as investigating the mechanisms by which binding is occurring. Sorption was found to be greatest in aromatic compounds across all three minerals used. Different organic compounds showed a slight preference for different minerals, but overall mineral type had a minimal effect on bonding. Organic compounds were found to bind cooperatively, achieving a higher organic matter: mineral ratio than the monolayer equivalent often observed in sediments. This suggest that the observed monolayer equivalence in marine sediments may be due to the nature and quantity of organic matter reaching these sediments rather than an inherent limit on the amount of organic matter that mineral surfaces can sorb. Experiments were also carried out using natural dissolved organic matter (DOM) under riverine and marine conditions to determine the impact of minerals on riverine DOM transport. The different DOM sources were found to have a minimal effect on the degree of sorption with salinity and mineral mass having the greatest effect. This observation suggests that much lower coverage was achieved for the DOM than for the standards, possibly due to the presence of a more limited range of compounds. Differences between the dissolved and standards data highlight the importance of including all compound types in the study of organic matter-mineral interactions. Given the complex nature of these interactions, and the different factors effecting them, further work is need to fully understand the role they play in organic matter preservation. However, this work has demonstrated the importance of careful experimental design, and the inclusion of both dissolved and particulate matter. Table of Contents Table of Contents Table of Contents .......................................................................................................... i Table of Tables ............................................................................................................. v Table of Figures ........................................................................................................... vii Research Thesis: Declaration of Authorship ................................................................ xiii Acknowledgements ..................................................................................................... xv Definitions and Abbreviations .................................................................................... xvii Chapter 1 Introduction ............................................................................................... 1 1.1 The global carbon cycle .............................................................................................. 1 1.1.1 Marine sediments .............................................................................................. 3 1.2 Organic matter-mineral interactions ......................................................................... 5 1.2.1 Clay minerals ...................................................................................................... 6 1.2.2 Iron minerals ...................................................................................................... 7 1.2.3 Organic matter ................................................................................................... 9 1.2.4 Mechanism ....................................................................................................... 10 1.3 Aim of this study ....................................................................................................... 10 Chapter 2 Materials and Methods ............................................................................ 13 2.1 Initial work ................................................................................................................ 13 2.1.1 Organic matter and mineral sources ................................................................ 13 2.1.2 Instrumentation ............................................................................................... 14 2.1.3 Analysis of starting materials ........................................................................... 15 2.1.4 Experimental set up ......................................................................................... 15 2.2 Standards work ......................................................................................................... 19 2.2.1 Organic matter and mineral sources ................................................................ 19 2.2.2 Instrumentation ............................................................................................... 21 2.2.3 Analysis of starting materials ........................................................................... 22 2.2.4 Experimental set up ......................................................................................... 24 2.3 CEH Work .................................................................................................................. 26 i Table of Contents 2.3.1 Organic matter and mineral sources ............................................................... 26 2.3.2 Instrumentation ............................................................................................... 27 2.3.3 Analysis of starting material ............................................................................ 28 2.3.4 Experimental set up ......................................................................................... 30 2.4 Conclusion ................................................................................................................ 31 Chapter 3 Importance of Organic matter type on the extent of organic matter-mineral sorption .................................................................................................... 33 3.1 Introduction ............................................................................................................. 33 3.2 Method .................................................................................................................... 33 3.3 Results and discussion ............................................................................................. 34 3.3.1 Individual compounds ...................................................................................... 34 3.3.2 Combined compounds ..................................................................................... 38 3.4 Conclusion ................................................................................................................ 48 Chapter 4 Mechanism of organic matter mineral bonding ......................................... 51 4.1 Introduction ............................................................................................................. 51 4.2 Material and Methods ............................................................................................. 52 4.3 Results and discussion ............................................................................................. 53 4.3.1 Ionic composition ............................................................................................. 53 4.3.2 Ionic strength ................................................................................................... 57 4.3.3 pH ..................................................................................................................... 62 4.3.4 Temperature .................................................................................................... 66 4.3.5 Implications for mechanism ...........................................................................
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